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A novel spin\u2010crossover (<jats:italic>SCO<\/jats:italic>) material based on iron(II) complexes incorporating 4\u2010acetylpyridine (4\u2010acpy) and [Hg(SCN)<jats:sub>4<\/jats:sub>]<jats:sup>2\u2212<\/jats:sup> anions was synthesized and formulated as [Fe(4\u2010acpy)<jats:sub>2<\/jats:sub>][Hg(<jats:italic>\u03bc<\/jats:italic>\u2010SCN)<jats:sub>4<\/jats:sub>] (<jats:bold>1<\/jats:bold>). Compound <jats:bold>1<\/jats:bold> is crystallized in a three\u2010dimensional network in the non\u2010centrosymmetric orthorhombic space group <jats:italic>Pna<\/jats:italic>2<jats:sub>1<\/jats:sub> with two octahedral [Fe(4\u2010acpy)<jats:sub>2<\/jats:sub>(NCS)<jats:sub>4<\/jats:sub>] entities featuring two distinct Fe centers (Fe1 and Fe2). Crystallographic, magnetic, and M\u00f6ssbauer measurements reveal an incomplete <jats:italic>SCO<\/jats:italic> exclusively at Fe2, with transition temperature <jats:italic>T<\/jats:italic><jats:sub>1\/2<\/jats:sub>\u2248102\u2005K. Photomagnetic studies conducted at 10\u2005K with lasers ranging from 405 to 1310\u2005nm evidence light\u2010induced excited spin\u2010state trapping (<jats:italic>LIESST<\/jats:italic>) and <jats:italic>reverse\u2010LIESST<\/jats:italic> effects, with a unique near\u2010infrared\u2010responsive <jats:italic>LIESST<\/jats:italic> phenomenon at 1064 and 1310\u2005nm. Advanced photocrystallographic studies at 40\u2005K provide precise structural evidence for these metastable states. The optical and vibrational properties consistently corroborate with magnetic and photomagnetic studies. Additionally, temperature\u2010 and light\u2010dependent terahertz (THz) absorptions are associated with phonon vibrations around Fe2 centers, through <jats:italic>SCO<\/jats:italic> behavior, as supported by ab initio calculation. The Fe(II)\u2212Hg(II) systems can be promising benchmarks for exploring synergistic switching effects in structural, magnetic, and spectroscopic properties.<\/jats:p>","DOI":"10.1002\/anie.202423095","type":"journal-article","created":{"date-parts":[[2024,12,11]],"date-time":"2024-12-11T08:32:28Z","timestamp":1733905948000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Near\u2010Infrared Light\u2010Induced Spin\u2010State Switching Based on Fe(II)\u2212Hg(II) Spin\u2010Crossover Network"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5168-7998","authenticated-orcid":false,"given":"Guanping","family":"Li","sequence":"first","affiliation":[{"name":"Department of Chemistry School of Science The University of Tokyo  7-3-1, Hongo Bunkyo-ku Tokyo, 113-0033 Japan"},{"name":"Department of Chemistry The University of Manchester  Manchester M13 9PL 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